Coal tar pitch (CTP), a by-product of coking industry, has a unique molecule structure comprising an aromatic nucleus and several side chains bonding on this graphene-like nucleus, which is very similar to the structure of graphene quantum dots (GQDs). Based on this perception, we develop a facile approach to convert CTP to GQDs only by oxidation with hydrogen peroxide under mild conditions. One to three graphene layers, monodisperse GQDs with a narrow size distribution of 1.7 ± 0.4 nm, are obtained at high yield (more than 80 wt. %) from CTP. The as-produced GQDs are highly soluble and strongly fluorescent in aqueous solution. This simple strategy provides a feasible route towards the commercial synthesis of GQDs for its cheap material source, green reagent, mild condition, and high yield.
Low-cost and earth-abundant coal has been considered to have a unique structural superiority as carbon sources of carbon quantum dots (CQDs). However, it is still difficult to obtain CQDs from raw coal due to its compactibility and lower reactivity, and the majority of the current coal-based CQDs usually emit green or blue fluorescence. Herein, a facile two-step oxidation approach (K2FeO4 pre-oxidation and H2O2 oxidation) was proposed to fabricate bandgap tunable CQDs from anthracite. The K2FeO4 pre-oxidation can not only weaken the non-bonding forces among coal molecules which cause the expansion of coal particles, but also form a large number of active sites on the surface of coal particles. The above effects make the bandgap tunable CQDs (blue, green, or yellow fluorescence) can be quickly obtained from anthracite within 1 h in the following H2O2 oxidation by simply adjusting the concentration of H2O2. All the as-prepared CQDs contain more than 30 at% oxygen, and the average diameters of which are <10 nm. The results also indicate that the high oxygen content only can create new energy states inside the band gap of CQDs with average diameter more than 3.2 ± 0.9 nm, which make the as-prepared CQDs emit green or yellow fluorescence.
The conventional synthesis route of graphene oxide (GOG), based on Hummers method, suffers from explosion risk, environmental concerns and a tedious synthesis process, which increases production costs and hinders its practical applications. Herein, we report a novel strategy for preparing few-layer graphene oxide (GOH) from humic acid via simple hydrothermal treatment. The formation of GOH is mainly attributed to the hydrolysis, oxidation and aromatization of humic acid under hydrothermal conditions. The as-prepared few-layer GOH has typical morphology (thin and crumpled sheets with the thickness of ~3.2 nm), crystal structure (a Raman ID/IG ratio of 1.09) and chemical composition (an X-ray Photoelectron Spectroscopy (XPS) O/C atomic ratio of 0.36) of few-layer GOG. The thermally reduced GOH (r-GOH) delivers considerable area capacitance of 28 µF·cm−2, high rate capability and low electrochemical resistance as supercapacitor electrodes. The described hydrothermal process shows great promise for the cheap, green and efficient synthesis of few-layer graphene oxide for advanced applications.